Formulations Containing Microencapsulated Essential Oils

ABSTRACT

A “green” agricultural formulation including at least one encapsulated volatile essential oil and a non-volatile vehicle in which the at least one encapsulated volatile essential oil is carried.

CROSS-REFERENCE TO RELATED APPLICATIONS

This application is a Continuation of U.S. patent application Ser. No.11/795,866 filed on Oct. 2, 2007 which is a National Stage ofInternational patent application PCT/IL2005/000705 filed on Jul. 4, 2005which designated the United States and claimed priority from U.S. patentapplication Ser. No. 11/040,102 filed on Jan. 24, 2005.

FIELD OF THE INVENTION

This invention relates to formulations containing microencapsulatedessential oils.

BACKGROUND OF THE INVENTION

Prior to the development of the modern chemical and pharmaceuticalindustries essential oils were used in many areas of daily life asantiseptic and disinfectant materials in pharmaceutical and cosmeticapplications such as antimicrobial and larvicidal agents. Essential oilbased formulations with a broad spectrum of antimicrobial activity havebeen shown to be relatively nontoxic to mammals. They have been replacedwith more potent synthetic chemicals and antibiotics, which are cheaperand highly effective and can be used in lower concentrations. With time,however, the toxicity and environmental effects of these syntheticchemicals have been revealed, and there is now an effort to replace themwith the same essential oil agents that they had originally replaced.

The use of such essential oil based formulations in agriculture has alsobeen reported. PCT Publication No. WO 04/098767 (Application No.PCT/IL2004/000394), to the inventors of the present application,disclose microcapsules of essential oils which may be used asdisinfectant products for the consumer market as hard-surface cleaners,laundry detergents and softeners, as pesticides, insect repellents, andas antiviral or antifungal agents. When the microcapsules are applied togiven substrates, the essential oil contained therein is released at aconstant rate over a period of time. The efficacy of such microcapsulesdepends solely on parameters relating to the microcapsules themselves,i.e., size, thickness of the encapsulating membrane, ability to sustainrelease of the essential oil contained therein, etc., and not on theaqueous medium which carries them to the target environment and whichdries immediately thereafter.

SUMMARY OF THE INVENTION

It has now been found, in accordance with the present application, thatthe efficacy of encapsulated volatile essential oils as pesticides,repellents, ovicides, larvicides and antiviral agents may increase ifthey are suspended or dispersed in a non-volatile vehicle, which maycontain such agents as high boiling or high melting essential oils andlipids. More specifically it has been determined that the efficacy ofthese encapsulated volatile oils increases, if, upon application to thesubstrate or target environment, they remain, for example, uponevaporation of an aqueous medium, in contact with a non-volatile agent,which is capable of enhancing the exerted effect. It has also beensurprisingly found that the effect of the non-volatile vehicle may beadditive or synergistic.

Thus, the present invention provides an agricultural formulationcomprising at least one encapsulated volatile essential oil and anon-volatile vehicle, in which said at least one encapsulated volatileessential oil is carried. The non-volatile vehicle may be a solid or aliquid vehicle.

The expression “encapsulated essential oil” or “encapsulation” or anylingual variation thereof refers herein to a granule of any shape andsize, which is capable of holding therein one or more essential oils.One example of such encapsulation is microencapsulation. Although theagricultural formulation of the present application, without affectingits benefits, may make use of any encapsulated essential oil granulesknown in the art, the preferred granule form is of a microcapsule. Thepreferred microcapsule is one having from 30 to 98%, or more preferablyfrom 60-95%, of its weight a volatile essential oil and which isprepared by interfacial polymerization of isocyanates. Suchpolymerization affords a microencapsulating shell of polyurethanes,polyureas or combinations thereof, as disclosed for example in WO04/098767. Such a microcapsule typically has an average size of between0.1 and 100 microns. Other suitable microcapsules may be prepared bysuch methods as disclosed for example in WO 94/13139, EP0252897, U.S.Pat. No. 5,576,009 and U.S. Pat. No. 5,925,464.

Thus, the present invention more specifically provides an agriculturalformulation comprising at least one microcapsule containing volatileessential oil, and a non-volatile vehicle.

The term “non-volatile vehicle” as used herein refers generally to anorganic agent that remains with the microcapsule on the targetenvironment after application and which exerts an additive orsynergistic effect. Such a vehicle may be a liquid or a solid (pure ormixture) having a high boiling or melting point and which rate ofevaporation from the surface of the target environment, afterapplication thereto, is smaller as compared to the encapsulatedessential oil. Such vehicles or carriers may for example be non-volatileessential oils, non-volatile botanical oils, non-volatile or solidterpenes, and lipids.

The vehicle is never water alone. However, in various embodiments it maybe necessary that water be the major component of the formulation. Insuch exemplary cases when the microcapsules are made in aqueoussolutions, or when water is added to allow better fluidity andsprayabillity or when the formulation is packaged or stored in water,the non-volatile vehicle may be added to the water solution which actsas a medium and has no beneficial effect on the repelling, insecticidal,pesticidal, larvicidal or ovicidal characteristics of the formulation.As it will be described hereinbelow, after application of theformulation, the water evaporates leaving behind the microcapsulesuspended in the non-volatile vehicle. In other embodiments, water maynot be necessary.

When said vehicle is a liquid essential oil or a lipid, the term refersto those having boiling points higher then 300.degree. C. Such highboiling point essential oils may for example be pyrethrins. An exampleof a lipid is sesame oil or cottonseed oil.

The term “solid vehicle” refers to a solid agent, pure or mixture, inwhich the microcapsules are admixed and which may be dissolved in,suspended in or dispersed evenly in a liquid medium, e.g. water, priorto application onto the target. Solid vehicles may for example be in theform of powders. The term “liquid vehicle” refers to a pure liquid, to ahomogeneous liquid mixture of agents (each of which before mixing may bea solid, a liquid, or a gas) or to a heterogeneous mixture of suchagents, e.g. suspension, in which said encapsulated essential oils e.g.,microcapsules may be suspended. The suspension of the microcapsules inthe liquid vehicle or in the solution prepared by dissolving ordispersing a solid vehicle in an appropriate medium, as for examplewater, should be such that the consistency, distribution, physicalstate, or concentration of the volatile essential oil within themicrocapsule is not affected. Such vehicle additionally is one in whichsaid microcapsules do not dissolve, deteriorate, decompose, leach out orundergo any other physical or chemical transformation. The term“suspended” or any other lingual variation thereof refers to a state ofdispersion of the microcapsules in the vehicle or a dispersion of themicrocapsules and vehicle in a non-miscible liquid; by way of anon-limiting example the dispersion is of cottonseed oil andmicrocapsules in water. The term may alternatively refer to a state ofcolloid, depending on the size of the microcapsules.

In one embodiment, said non-volatile vehicle is at least onenon-volatile essential oil, at least one non-volatile botanical oil orany combination thereof. Such combinations may for example be, withoutbeing limited thereto: (a) a combination of two or more differentnon-volatile essential oils; (b) a combination of two or more differentnon-volatile essential oils with at least one botanical oil; (c) acombination of one non-volatile essential oil with one non-volatilebotanical oil; (d) a combination of two different non-volatile botanicaloils, and the like. Similar variations may also be made with any onespecific sub-group, e.g. lipids and with any one specific representativethereof, as for example different triglycerides.

The terms “volatile”, “moderately volatile” and “non-volatile” refer tothe degree of evaporative ability of the chemical agent under ambienttemperature and pressure. Typically, the lower the agent's boiling pointis the more volatile the agent is said to be. In reference to essentialoils, the volatile, low boiling point oils are those defined as havingboiling points lower than about 250.degree. C. The moderately volatileoils are those defined as having boiling points of between 250.degree.C. and 300.degree. C. The non-volatile or less volatile oils are thosedefined as having boiling points higher than 300.degree. C.

“Botanical oils” are natural complex mixtures of oils made by plants.“Essential oils” are those that in general give to the plants theircharacteristic odors, flavors, or other such properties. Botanical oilsare found in various parts of the plant body (in the seeds, flowers,bark, or leaves) and are also concentrated in certain special cells orgroups of cells (glands). In general, they are complex mixtures that maybe obtained from the plant in various ways, depending upon the nature ofthe part in which they are found. Such methods may for example be bycompression, by distillation with steam, by dissolving the oils out(extraction) or absorbing them, and by pressure and maceration. The termalso refers to oil mixtures prepared by enriching naturally obtainedbotanical oil with one or more specific component such as monoterpenes,diterpenes, triterpenes, tetraterpenes, sesquiterpenes, and otherpolyterpenes as well as organic alcohols, aldehydes ketones, acids andesters.

While the terms “essential oils” and “botanical oils” are used indifferent literary sources interchangeably, within the scope of thepresent invention the latter refers to a larger group of compounds thatalso includes lipids.

“Lipids” as referred to herein include the fatty, acids, theglycerol-derived lipids (including the fats and oils and thephospholipids), the sphingosine-derived lipids (including the ceramides,cerebrosides, gangliosides, and sphingomyelins), the steroids and theirderivatives, the terpenes and their derivatives, certain aromaticcompounds, and long-chain alcohols and waxes. The term also refers tolipoproteins (lipids conjugated with proteins or carbohydrates), tolipopolysaccharides and to vitamins such as fat-soluble vitamins.

In a preferred embodiment, the botanical oils are selected from sesameoil, pyrethrum, glycerol-derived lipids or glycerol fatty acidderivatives and the said at least one encapsulated essential oil isselected from cinnamon, cedar, dove, geranium, lemongrass, mint, sesame,thyme oil, turmeric oil, wintergreen oil, rosemary, anise oil, cardamomoil, chamomile oil, coriander oil, cumin oil, dill oil, mint oil,parsley oil, basil, camphor, citronella, eucalyptus, fennel, ginger,grapefruit, lemon, mandarin, orange, pine needle, pepper oil, rose oil,sweet orange oil, tangerine, tea tree, tea seed, caraway, garlic,peppermint oil, onion, and spearmint oil. Preferably, essential oils arevolatile and may be chosen without limitation from citronella, geranium,tea tree, lavender, clove pine and eucalyptus.

In another embodiment of the present invention, the formulations of thepresent invention may also comprise adjuvants, adhesives, antioxidants,water-resistant agents, surfactants, steric barrier polymers whichprevent microcapsule aggregation and gel-breaking agents, as part of thevehicle or within the microcapsule.

Adjuvants may be used for example to improve shelf life, sprayabillity,and adsorption to the substrate. Such adjuvants may be chosen from bothnatural and synthetic polymers such as polyvinyl alcohol,polyvinylpyrrolidone, polyethylene oxides, ethylene or maleic anhydridecopolymers, methyl vinyl ether-maleic anhydride copolymer, water-solublecellulose, water soluble polyamides or polyesters, copolymers orhomopolymers of acrylic acids, water-soluble starches and modifiedstarches, natural gums such as alginates, dextrins and proteins such asgelatins and caseins.

In another embodiment, the formulation may also comprise pesticides suchas insect growth regulators (IGR), herbicides, insecticides, acaracides,fungicides, nematicides, ectoparasiticides, and/or herbicides eitherwithin the microcapsule or as part of the vehicle. Preferably, saidformulation may contain pesticides which are soluble in either said atleast one encapsulated essential oil or in the non-volatile vehicle.Such pesticides may for example be carbamates, ureas, triazines,triazoles, uracils, organophosphates, morpholines, dinitroanilines,acylalaninies, pyrethroids, and organochlorines. Specific examples arecarbofuran, azinphos-methyl, sulfentrazone, carfentrazone-ethyl,cypermethrin, cyromazine, beta-cyfluthrin, endosulfan, phosmet,chlorobromuron, chloroxuron, chlorotoluron, fluometuron, metobromuron,thiazafluron, teflubenzuron, hexaflumuron, diflubenzuron, flufenoxuron,lufenuron, chlorfluazuron, novaluron, dimethachlor, metolachlor,pretilachlor, 2-chloro-n-(1-methyl-2-methoxyethyl)-acet-2,6-xylidide,alachlor, butachlor, propachlor, dimethenamid, bifenox,4-(4-pentyn-1-yloxy)diphenylether, acifluorfen, oxyfluorfen,fluoroglycofen-ethyl, fomesafen,cis,trans-(+)-2-ethyl-5-(4-phenoxyphenoxymethyl)-1,3-dioxolane,fluazifop-butyl, haloxyfop-methyl, haloxyfop-(2-ethoxyethyl),fluorotopic, fenoxapropethyl, quizalofop-ethyl, propaquizafop,diclofop-methyl, butralin, ethalfluralin, fluchloralin, isopropalin,pendimethalin, profluralin, trifluralin, imidocloprid, aclalaninesfuralaxyl, metalaxyl, benzoylprop ethyl, flamprop methyl,difenoconazole, etaconazol, propiconazole,1,2-(2,4-dichlorophenyl)-pent-1-yl-1h-1,2,4-triazole, triadimefon,dioxacarb, furathiocarb, aldicarb, benomyl, endosulfan,2-sec-butylphenylmethylcarbamate, etiofencarb, fenoxycarb, isoprocarb,propoxur, carbetamid, butylate, di-allat, eptc, molinate, thiobencarb,tri-allate, vemolate, piperophos, anilofos, butamifos, azamethiphos,chlorfenvinphos, dichlorvos, diazinon, methidathion, azinphos ethyl,azinphos methyl, chlorpyrifos, chlorthiofos, crotoxyphos, cyanophos,demeton, dialifos, dimethoate, disulfoton, etrimfos, famphur,flusulfothion, fluthion, fonofos, fomothion, heptenophos, isofenphos,isoxathion, malathion, mephospholan, mevinphos, naled, oxydemetonmethyl, oxydeprofos, parathion, phoxim, pyrimiphos methyl, profenofos,propaphos, propetamphos. prothiophos, quinalphos, sulprofos, phemephos,terbufos, triazophos, trichloronate, fenamipos, isazophos,s-benzyl-o,o-diisopropylphosphorothioate, edinphos, and pyrazophos.

The physical state of the formulation, namely as a solid or liquid,depends on whether the non-volatile vehicle is a liquid or a solid orwhether the non-volatile vehicle and microcapsules are suspended ordispersed in an immiscible liquid such as water. Regardless of itsphysical state, the formulation may be put to use by further forming itinto a desirable preparation form, such as an emulsifiable concentrate,a wettable powder, a granular wettable powder, a flowable preparation, asuspension, a granule, a dust, a fumigant and the like. The nature ofthe preparation form may be decided based on such parameters as thetarget environment, the method of application, the conditions underwhich the application is performed, the relative concentration of themicrocapsules in the non-volatile vehicle, etc.

Although the concentration of the microcapsules in the non-volatilevehicle may be controlled, the concentration of the encapsulatedessential oil may vary depending on storage, climate conditions,preparation form, method of application, place of application, objectivepests to be controlled, objective crop plant, and the like. Theconcentration of volatile essential oils within a formulation may varybetween 0.01 to 90%, or preferably from 0.1 to 25%. With respect toapplications to the target environment, e.g. a crop field, the volatileessential oils may be appropriately selected from a range of 0.1% andpreferably 0.25% in terms of weight of volatile essential oil, perfield.

Without wishing to be bound by theory, when, for example, an aqueousbased formulation is applied to the target environment, the watertherein dries on the surface, leaving a layer of the non-volatilevehicle in which the encapsulated volatile essential oils are embedded.The initial effect on the treated environment is exerted by thenonvolatile vehicle; slowly thereafter, be it through spontaneousrelease or by any other initiated release, the microcapsules beginreleasing their content, thereby both affecting either an additive orsynergistic effect on the environment.

The formulations of the present invention may be adaptable to the fourprofiles of microcapsule release, namely (1) a rapid release profile;(2) a sustained or a delayed release profile; (3) a so-called“knock-down” biological effect profile under which the microcapsulereleases its content as one portion or over a relatively short time; and(4) a residuality profile in which the so-called “knock-down” isfollowed by a sustained release profile.

The formulation of the present invention may be used for variousagricultural, horticultural and agronomic purposes dependent on thespecific essential oils used. The term “agricultural formulation” alsorefers to horticultural and agronomic formulations. Without wishing tobe bound by theory and modes of operation, the formulations may act asrepellents by driving the pests off without ensuing their death; asinsecticides (or pesticides) by killing a part of or a whole populationof insects or other pests; and as ovicides by killing a part or a wholepopulation of insect eggs. The term “pest” refers also to insects,nematodes, and to any other injurious animal to humans, animals andplant varieties. Examples of pests are those belonging to theheteroptera of hemiptera, homoptera, coleoptera, leopidoptera,thysanoptera, hymenoptera, isoptera, orthoptera, acarina, dolylamida,gstopoda and tylenchida.

Examples for pests belonging to heteroptera are plataspid bug (Megacoptapunctatissimum), whitespotted bug (Eysarcoris parvus), southern greenstinkbug (Nezara viridula), brownwinged green bug (Plautia stali), ricebug (Leptocorisa chinensis), bean bug (Riptortus clavatus), rice leafbug (Togo hemipterus), pear lace bug (Stephanitis nashi), azelea lacebug (Stephanitis pyrioides), pale green plant bug (Apolygus spinolai),narrow squash bug (Cletus puctiger), sorghum plant bug (Stenotusrubrovittalus), whitespotted larger spined bug (Eysarcoris lewisi) andrice leaf bug (Trigonotylus coelestialium).

Examples of pests belonging to coleoptera are cupreous chafer (Anomalacuprea), powderpost beetle (Lyctus brunneus), confused flour beetle(Tribolium confusum), twenty-eight-spotted ladybird (Epilachnavigintioctopunctata), Japanese beetle (Popillia japonica), whitespottedlongicom beetle (Anoplophora malasiaca), Japanese pine sawyer(Monochamus alteratus), azuki bean weevil (Callosobruchus chinensis),rootworm (Diabrotica spp.), boll weevil (Anthonomus grandis grandis),pepper weevil (Anthonomus eugenii), cucurbit leaf beetle (Aulacophorafemoralis), Mexican beetle (Epilachna varivestis), Colorado leaf beetle(Leptinotarsa decemlineata), rice water weevil (Lissorhoptrusoryzophylus), rice leaf beetle (Oulema oryzae), and hunting billbug(Sphenophrus venatus vestitus).

Examples of pests belonging to homoptera are leafhopper (Arboridiaapicalis), tea green leafhopper (Empoasca onukii), green rice leafhopper(Nephotettix cincticeps), green rice leafhopper (Nephotettix virescens),small brown planthopper (Laodelphax striatellus), brown rice planthopper(Nilaparvata lugens), whitebacked rice planthopper (Sogatellafurcifera), citrus psylla (Diaphorina citri). citrus spiny whitefly(Aleurocanthus spiniferus), silverleaf whitefly (Bemisia argentifolli),sweetpotato whitefly (Bemisia tabaci), citrus whitefly (Dialeurodescitri), grapeleaf louse (Viteus vitifolli), woolly apple aphid (Eriosomalangierum). red scale (Aonidiella aurantii), cowpea aphid (Aphiscraccivora), greenhouse-potato aphid (Aulacorthum solani), cabbage aphid(Brevicoryne brassicae), potato aphid (Macrosiphum euphorbiae),greenhouse whitefly (Trialeurodes vaporariorum), green peach aphid(Myzus persicae), oat bird-cherry aphid (Rhopalosiphum padi), japanesegrain aphid (Sitobion akebiae), comstock mealybug (Pseudococcuscomstocki), Inidan wax scale (Ceroplastes ceriferus), mulberry scale(Pseudaulacapsis pentagoa), cotton aphid (Aphis gossipii), andarrowedhead scale (Unaspis yanonensis).

Examples of pests belonging to lepidoptera are summer fruit tortrix(Adoxophyes orana fasciata), smaller tea tortrix (Adoxophyes honmai),apple tortrix (Archips fuscocupreanus), oriental fruit moth (Grapholitamolesta), oriental tea tortrix (Homona magnanima), tea leafroller(Caloptilia theivora), mugwort looper (Ascotis selenaria), grape berrymoth (Endopiza viteana), codling moth (Laspeyresia pomonella), appleleafminer (Phyllonorycter ringoniella), apple leaf miner (Lyonetiaprunifoliella malinella), diamondback moth (Plutella xylostella), pinkbollworm (Pectinophora gossypiella), peach fruit moth (Carposinaniponensis), peach fruit moth (Carposina niponensis), rice stem borer(Chilo supperssalis), citrus leafminer (Phyllocnistis citrella), yellowrice borer (Scirpophaga incertulas), rice leafroller (Cnaphalocrosismedinalis), cabbage webworm (Hellulla undalis), Chinese yellowswallowtail (Papilio xuthus), common white (Pieris rapae crucivora),fall webworm (Hyphantria cunea), bluegrass webworm (Parapediasiatererrela), corn earworm (Helicoverpa armigera), cutworm (Agrotissegetum), beet semi-looper (Autographa nigrisigna), cabbage armyworm(Mamestra brassicae), beat armyworm (Spodoptera exigua), Heliothis(Heliothis spp.), and common cutworm (Spodoptera litura).

Examples of pests belonging to hymenoptera are cabbage sawfly (Athaliarosae ruficomis), rose argid sawfly (Arge pagana), and Formica japonica.Examples of pests belonging to diptera are rice leafminer (Agromyzaoryzae), rice leafminer (Hydrellia griseola), legume leafminer(Liriomyza trifolii), onion maggot (Delia antiqua), house fly (Muscadomestica), Culex pipiens molestus, and house mosquito (Culex pipienspallens).

Examples of pests belonging to thysanoptera are yellow tea thrips(Scirtothrips dorsalis), southern yellow thrips (Thrips palmi), onionthrips (Thrips tabaci), and western flower thrips (Frankliniellaoccidentalis).

Examples of pests belonging to isoptera are Formosan subterraneantermites (Coptotermes formosamus), japanese subterranean termite(Reticulitermes speratus); and examples of pests belonging to Psocopteraare booklice (various spp.), and Liposcelis bostrychophilus.

Examples of pests belonging to orthoptera are rice grasshopper (Oxyayezoensis), mole crichet (Gryllotalpa sp.), American cockroach(Periplaneta americana), and German cockroach (Blatella germanica).

Examples of pests belonging to acarina are citrus red mite (Panonychuscitri), two-spotted spider mite (Tetranychus urticae), broad mite(Polyphagotarsonemus latus), southern false spider mite (Brevipalpusphoenicis), clover mite (Bryobia praetiosa), pink citrus rust mite(Aculops pelekassi), japanese pear rust mite (Eriophyes chibaensis),bulb mite (Rhizoglyphus robini), fruit tree red spider mite (Panonychusulmi), and mold mite (Tyrophagus putrescentiae).

Examples of pests belonging to tylenchida are coffee root-lesionnematode (Pratylenchus coffeae), Cobb root-lesion nematode (Pratylenchuspenetrans), potato cyst nematode (Globodera rostochiensis), and southernroot-knot nematode (Meloidogyne incognita). An example of pestsbelonging to dolylamida is the needle nematode (Longidorus sp.) and anexample of pests belonging to gastropoda is the slug (Incilariabilineata).

By effecting the population of insects capable of inflicting damage tothe target environment, the formulations may also assist in reducingdamage caused by plant viruses, by limiting viral transmission by insectvectors. The most severe damage to target environments occurs throughthe transmission of plant viruses, primarily begomoviruses, one of themost damaging of which on tomato is the Tomato yellow leaf curl virus(TYLCV).

It has also been found in the course of the investigation leading to theinvention of the present application, that the non-volatile vehicleenhances the repelling, insecticidal, pesticidal, ovicidal or antiviraleffect exerted by the volatile essential oil, and that the effectexerted by the non-volatile vehicle is enhanced by the volatileessential oil.

Thus, the present invention further provides repellent, insecticidal,pesticidal, ovicidal and antiviral formulations comprising each aneffective amount of the formulation of the present invention.

In one embodiment, the formulation may be used as an insect repellentagainst such insects as the silverleaf whitefly, and as ovicides againstsuch pests as white fly, tomato pinworm and pepper weevil pests.

In one specific embodiment, there is provided a repellent formulationagainst the whitefly, said formulation comprises encapsulated citronellaoil and/or geranium oil and/or tea tree oil and/or lavender oil and/orclove oil and a liquid vehicle comprising pyrethrum and sesame oil.

In another specific embodiment, the formulation against the whiteflycomprises encapsulated ginger oil and a liquid vehicle comprisingcottonseed oil.

In yet another specific embodiment, there is provided a repellentformulation against the tomato pinworm Keiferia lycopersicella (Wals.),said formulation comprises citronella oil and/or geranium oil and/or teatree oil and/or lavender oil and/or clove oil and a liquid vehiclecomprising pyrethrum and sesame oil.

In another embodiment, there is provided an ovicidal or repellentformulation against the pepper weevil, Anthonomus eugenii Cano, saidformulation comprises citronella oil and/or geranium oil and/or tea treeoil and/or lavender oil and/or clove oil and liquid vehicle comprisingpyrethrum and sesame oil.

In another embodiment, the formulation of the present invention may beused against viral transmitting pests capable of acting as viral vectorsfor infection. The term “viral vector” refers to any such pest asdefined and exemplified herein which is capable of carrying andtransmitting a plant virus disease-causing, organism.

As stated herein before, the formulation of the present invention makesuse of any essential oil contained in microcapsules that may be preparedby any known method. The microcapsules, which are thus prepared, may beeither recovered from the reaction mixture and re-suspended in saidnon-volatile vehicle or in a solution containing thereof. Alternatively,any medium, aqueous or otherwise, which comprises the microcapsules, maybe treated without initial separation from the medium in which they aremanufactured with at least one non-volatile vehicle. In most cases saidmedium is water.

In cases where separation is preferred, the recovery of themicrocapsules may be achieved, depending on their size, bycentrifugation or filtration and washed with several portions of anappropriate solvent, e.g. distilled water, to remove free reactants fromthe surface. If necessary, the microcapsules may be heated under reducedpressure to further remove any residual reactants from within themicrocapsules. Preferably, this procedure is carried out by heating themicrocapsule at a temperature above the median glass transitiontemperature of the polymer making up the microcapsule shell.

These microcapsules may now be dispersed or suspended in saidnon-volatile liquid or solid vehicle. In some cases, said non-volatilevehicle is a particulate solid, e.g. powder, by which the dispersion ispreferably done by admixing an effective amount of dry microcapsuleswith said vehicle. In some cases, said non-volatile vehicle is a liquid,by which the suspension is preferably prepared by mechanically stirringan effective amount of the microcapsules in said vehicle. The term“effective amount” as used herein refers to an amount determinedempirically, which exerts on the target environment the desired effectas is described herein below.

Thus, the present invention further provides a method for themanufacture of the formulation of the present invention, said methodcomprising dispersing at least one encapsulated essential oil in anon-volatile vehicle or in a medium containing thereof.

The present invention additionally provides a method for the manufactureof the formulation of the present invention, said method comprisingadding to any aqueous preparation of encapsulated volatile essentialoils an amount of a non-volatile vehicle, as defined hereinabove.

The “aqueous preparation of encapsulated volatile essential oils” is apreparation manufactured by any process known to a person skilled in theart. Preferably said aqueous preparation of encapsulated volatileessential oils is a preparation manufactured in accordance with theprocess claimed in WO04/98767, said process comprising generallydissolving a di- or polyisocayante into an essential oil, emulsifyingthe resulting mixture in an aqueous solution containing a di- orpolyamine, and/or a di- or polyhydroxy compound to effect encapsulationof said essential oil through interfacial polymerization, whereby thereis formed a polyurea and/or polyurethane film around the essential oildroplets, which film enhances the stability of said essential oil,reduces its evaporation rate and controls its release rate when appliedto a substrate.

Once manufactured, the liquid or solid formulation (e.g., solublesolids) may be preserved until it is released by some means into theenvironment. Often it is most convenient to bottle or can the suspensioncontaining the encapsulated essential oil, in which case it may bedesirable to add formulation adjuvants to the formulation. “Formulationadjuvants” such as density balancing agents, surfactants, thickeners,biocides, dispersants, antifreeze agents, salts, and the like may beadded to improve suspension stability and the ease of application. Sucha formulation adjuvant may be added to the suspension of microcapsulesat a concentration of from about 0.01% to about 30% by weight of thesuspension.

The method for the manufacture of the formulation may include alsoadding to the liquid vehicle or to the medium, e.g. water, containing itan ionic or non-ionic surfactant. Such surfactant may be added duringmanufacture of the microcapsules in order to facilitate or control thesize of the microcapsules and/or may be added after the microcapsulesare manufactured in order to break up a gel that results from themicroencapsulation and afford a flowable non-gel formulation. Oneespecially preferred surfactant is sodium dodecyl sulfate (SDS). It maypreferably be added in concentrations of 0.1 to 10% and most preferablyin concentrations of 0.5% to 5%.

Other non-limiting examples of preferred additives in addition tosurfactants are steric barrier polymers, which help maintain particleseparation, such as polyvinylpyrrolidone (PVP), polyvinyl alcohol (PVA)and poly(ethoxy)nonylphenol. In some cases it is desirable to adjust thepH of the finished microcapsule formulation as, for example, when thesolution of finished microcapsule is combined with other pesticides.Conventional reagents for adjustment of acidity or alkalinity, may beused, including for example, hydrochloric acid, sodium hydroxide, sodiumcarbonate, and sodium bicarbonate.

In another aspect of the present invention, there is provided a methodfor managing pest population, said method comprising applying to thetarget environment or to said pest population or to the loci thereof,the formulation of the present invention.

By “managing pest population” it is meant one or more of the following:driving off a part of or a whole pest population from a selected targetenvironment; controlling future generations; extermination of a part ofor a whole pest population; eliminating breeding places; exposing targetenvironment before infestation to the repellent or insecticideformulation; limiting adult, larvae or pest eggs prior to infestation orafter infestation has caused damage; and reducing signs of damage. Theterm “pest population” refers to an adult pest population, larval ornymphal population, egg population, mixed populations, or anycombinations thereof, wherein the number of pests in the population mayvary from one to several millions.

The term “target environment” as used herein refers to both primaryenvironments, which are susceptible to injury by pest population, and tosecondary environments, which surround the primary environments andwhich do not include any agriculturally or horticulturally desirabletarget. Primary environments are, for example, leaves, bark, fruit,flowers, seeds, or roots of cereals such as rice, barley, wheat, rye,oat, corn, etc.; beans and peas such as soybean, red bean, broad bean,pea, kidney-bean, peanut, etc.; fruit trees such as apple, citrus, pear,grape, peach, plum, cherry, walnut, chestnut, almond, banana,strawberry, etc.; leafy and fruiting vegetables such as cabbage, tomato,spinach, broccoli, lettuce, onion, stone-leek, Spanish paprika,eggplant, pepper, etc.; root crops such as carrot, potato, sweet potato,taro, radish, lotus rhizome, turnip, burdock, garlic, etc.; processingcrops such as cotton, flax, beet, hop, sugarcane, sugar beet, olive,gum, coffee, tobacco, tea, etc.; cucurbitaceous plants such as pumpkin,cucumber, muskmelon, watermelon, melon, etc.; pasture plants such asorchard grass, sorghum, timothy, clover, alfalfa, etc.; lawn grasses;perfumery crops; flowers and ornamental plants; garden-trees such asginkgo tree, cherry tree, gold-leaf plant, etc.; and timber woods suchas white fir, silver fir, pine, hatchet-leaved arbor-vitae, Japan cedar,Japanese cypress, etc.

The target environment may also be a certain pest population againstwhich the formulation may be employed.

In order to control various pests, the formulation of the presentinvention may be applied to the plants on which appearance of the pestis expected, either as it is or in the form of a dilution or suspensionin a proper quantity of water or the like at a concentration effectivefor the control of the pest population. For instance, for controllingthe appearance of pests on edible agriculture products such as fruittrees, cereals and vegetables, the formulation may be used on thesurroundings and not directly on the target environment. The formulationmay also be adaptable for foliage treatment, seed treatment such asimmersion of seeds in the formulation for seed coating, incorporationinto the soil, drenching-in-hole treatment, nursery box application,etc.

The formulation of the present invention may be presented, stored,packed or applied as a single formulation, wherein the encapsulatedvolatile essential oil is pre-mixed with the non-volatile vehicle, or asa two-component formulation, which comprises the encapsulated volatileessential oil as one component, for example in a separate container orapplied separately, and the non-volatile vehicle as a second component.

Thus, there is provided a method for managing pest population, saidmethod comprising:

-   -   applying to the target environment a microcapsule formulation        comprising at least one volatile essential oil, and    -   applying to the target environment a second formulation        comprising a non-volatile agent.

The application of the second formulation may be done immediately afterthe application of the first formulation, or at any time thereafter. Aperson skilled in the art would be able to decide which of the twomethods of managing pest populations disclosed herein is more suitablefor the specific case.

The formulation of the present invention may be delivered into thetarget environment by any method known to a person skilled in the art.Such methods may include for example: (a) manual or mechanicalapplication of the formulation to the soil by, for example, applying aliquid preparation either diluted or undiluted with water to the plantbase; (b) applying a granular agent such as dust or a wettable powder tothe plant base, planting hole or planting row; (c) ground or aerialspraying of a liquid formulation to the whole field or to specificallyselected areas; (d) buying the formulation in the topsoil, etc. Theformulation may be applied on pre- or post-harvested fruits andvegetables and may additionally be applied on stored grain pests, housepests, sanitary insect pests and forest pests. Further, the applicationmay also be to construction material of house, using fumigation, bait,etc.

The mode of release of the essential oil from the microcapsule and theensued effect on the treated environment depends on the physicalcharacteristics of the microcapsule. In accordance with the presentinvention, the active volatile essential oil is a liquid depotencapsulated by the microcapsule membrane and carded in a non-volatilevehicle, which enhances, either additively or synergistically, itsexerted effect. Upon delivery of the formulation to the targetenvironment, the release of the microcapsule's content when applied tothe substrate is believed to commence due to the concentration gradientof the volatile essential oils inside and outside of the microcapsule.This release process and its kinetics may be influenced by:

-   -   (a) drying of the microcapsules;    -   (b) contact with an aqueous media, e.g. water or rain, which        causes slow decomposition of the microcapsule shell;    -   (c) high temperatures; and    -   (d) direct sun light. It may, however, be the case that none of        these conditions are required or have any effect on any        initiation, as the release of the microcapsule content may be        spontaneous and independent.

The formulation may also be used for managing pest populations in smallgardens, house nurseries, vegetable and flowerbeds, and on few specificspecimens such as houseplants.

There is, thus, provided a kit or a commercial package comprising theformulation of the present invention.

The present invention also provides a two-component kit comprising afirst container contained therein a suspension of at least oneencapsulated volatile essential oil and a second container containedtherein a non-volatile vehicle. Optionally, the kits of the presentinvention may also comprise instructions how to apply the two componentsto the target environment as to achieve the desirable effect.

The kit formulation or single component formulations may be presented ina solid or a liquid form and in concentrated or diluted state and may beapplied to the target environment by, for example, a sponge or a pieceof cloth, which was pre absorbed by the formulation, or by hand-heldspray.

The invention will now be described by way of examples with reference tothe accompanying Figures. While the forgoing description describes indetail only a few specific embodiments of the invention, it will beunderstood by those skilled in the art that the invention is not limitedthereto and that other formulations comprising encapsulated essentialoils and non-volatile vehicles may be applied to other types of pestsand for other purposes, without departing from the scope of theinvention as defined by the appended claims.

DETAILED DESCRIPTION OF THE INVENTION Example 1 Repellent FormulationsAgainst the White Fly, Tomato Pinworm and Pepper Weevil

Formulation 1: Formation of essential oil microcapsules is typicallycarried out by interfacial polymerization. For example in one case, 17.5g TDI (toluene diisocyanate) is mixed into 125 g citronella oil, whichis added into 250 g water containing 2.5 g PVA using a high sheer mixer.To this is added 70 ml of water with 27.8 g PEG 4000. The mixing iscontinued for two hours at room temperature. To this dispersant areadded 0.4 g of a xanthane gum (rodopol) and 2 g of a fungicide(nefocide). To break up the hydrogel character of this emulsion, 5 g SDS(sodium dodecyl sulfate, 1%) is added.

To this suspension of microcapsules in water are now added 10 g ofPyrethrum oil (50% concentrate) and 1 g sesame oil for every 89 g ofsuspension.

This general procedure was used to prepare a large number of otherrepellent formulations, hereon referred to as Formulations 2 to 15.

Formulation 2: This formulation was prepared similarly to Formulation 1using 93 g citronella oil, 10 g Pyrenthrum and 1 g sesame oil.

Formulation 3: This formulation was prepared similarly to Formulation 1using geranium oil as the encapsulated volatile essential oil.

Formulation 4: This formulation was prepared similarly to Formulation 1using tea tree oil as the encapsulated volatile essential oil.

Formulation 5: This formulation was also prepared similarly toFormulation 1 using lavender oil or clove oil as the encapsulatedvolatile essential oils.

Formulation 6: This formulation was prepared similarly to Formulation 1using 24.3 ml cottonseed oil and 0.62 ml encapsulated ginger oil.

Formulation 7: This formulation was prepared similarly to Formulation 1using 23.7 ml cottonseed oil and 1.25 ml encapsulated ginger oil.

Formulation 8: This formulation was prepared similarly to Formulation 1using 22.5 ml cottonseed oil and 2.5 ml encapsulated ginger oil.

Formulation 9: This formulation was prepared similarly to Formulation 1using 21.2 ml cottonseed oil and 3.7 ml encapsulated ginger oil.

Formulation 10: This formulation was prepared using the followingingredients and quantities in a process essentially identical to thatdisclosed for Formulation 1 above: 25 g PVA, 250 g ginger oil, 35 g TDI,55.6 g PEG 4000, 4 g Nefocide, 10 g SDS and 0.8 g Rodopol.

Formulation 11: This formulation was prepared using the followingingredients and quantities in a process essentially identical to thatdisclosed for Formulation 1 above: 2.1 g PVA, 110 g ginger oil, 10.1 gTDI, 12.5 g PEG 2000, 1.8 g Nefocide and 0.8 g Rodopol.

Formulation 12: This formulation was prepared using the followingingredients and quantities in a process essentially identical to thatdisclosed for Formulation 1 above: 2.0 g PVA, 90 g ginger oil, 3.5 gTDI, 0.8 g EDA, 0.7 g EDTA, 1.3 g Nefocide and 1.2 g Rodopol.

Formulation 13: This formulation was prepared using the followingingredients and quantities in a process essentially identical to thatdisclosed for Formulation 1 above: 2.1 g PVA, 88 g ginger oil, 22 gparaffinic oil, 10.1 g TDI 24.4 g PEG 4000, 1.8 g Nefocide and 0.5 gRodopol.

Formulation 14: This formulation was prepared using the followingingredients and quantities in a process essentially identical to thatdisclosed for Formulation 1 above: 2.1 g PVA, 88 g ginger oil, 22 gcottonseed oil, 15.3 g TDI, 24.4 g PEG 4000, 1.8 g Nefocide and 0.5 gRodopol.

Formulation 15: This formulation was prepared using the followingingredients and quantities in a process essentially identical to thatdisclosed for Formulation 1 above: 2.1 g PVA, 88 g ginger oil, 22 gsesame oil, 22 g TDI, 24.4 g PEG 4000, 1.8 g Nefocide and 0.5 g Rodopol.

Example 2 Application of Repellent Formulations onto a TargetEnvironment

The above formulations were tested on adult silverleaf whiteflies andeggs thereof. The following solutions were used as controls:

-   -   1. Water    -   2. Ultra-Fine Oil-a commercial product containing paraffinic        oil, and    -   3. Pyrethrum.

Various leaves of tomato seedlings were treated, top or bottom, with oneof the formulations prepared above, and the efficacy of the formulationas a repellent was measured based on the number of whitefly adultsrepelled therefrom, and based on the number of eggs laid on said treatedleaf. Generally speaking, and as may be noted from the below Tables, theefficacy of the formulations were much higher in comparison to the 3controls used. Furthermore, long-term tests showed that the controls hadno substantial effect.

Table 1 shows that Formulation 1 was effective in repelling thewhitefly, both in terms of the number of flies which landed on thetreated leaf and in terms of the number of eggs laid. For example, asmay be noted from Replica 1 of Table 1, the number of flies reducedoverall (leaf top+bottom) by 87% from 29 to 4 as compared to a reductionof 50% when treated with Ultra-Fine alone.

Similar results were observed also for Formulations 3 and 4, as shown inTable 2 (some of which are not shown therein).

TABLE 1 Effect of Formulation 1 on the Silverleaf Whitefly. UntreatedLeaf Treated Leaf Untreated Leaf Treated Leaf Untreated adult Treatedadult Formulation Top Bottom Top Bottom (# of eggs laid) (# of eggslaid) (leaf area) (leaf area) REPLICA 1 Ultra-Fine 0 0 8 672 323 260 240Pyrethrum 0 14 0 10 381 341 213 199 Water 0 18 0 28 579 303 232 201Form. 1 0 29 0 4 696 89 230 225 REPLICA 2 Ultra-Fine 0 35 1 13 403 93159 155 Pyrethrum 0 27 0 14 184 101 203 192 Water 0 30 0 17 302 183 170158 Form. 1 0 39 0 3 224 14 219 201 REPLICA 3 Ultra-Fine 0 12 0 4 572233 187 131 Pyrethrum 0 8 0 0 565 1 170 135 Water 0 6 0 8 466 297 183143 Form. 1 0 7 0 1 343 4 143 118

TABLE 2 Effect of Formulations 3 and 4 on the White fly. UNTREATEDTREATED Formulation ADULTS Leaf Area ADULTS Formulation No. Top BottomEGGS (cm²) Top Bottom EGGS Leaf Area REPLICA 1 Ultra-Fine 0 4 243 85.180 3 167 126.33 Pyrethrum 0 3 47 57.59 0 3 139 88.61 Water 0 2 114 68.760 8 172 77.44 Formulation 3 0 3 95 100.83 0 0 29 119.64 REPLICA 2Ultra-Fine 0 4 117 69.07 0 3 108 32.95 Pyrethrum 0 7 224 50.33 0 7 20251.06 Water 0 5 238 62.27 0 11 384 66.37 Formulation 3 0 11 335 81.22 00 58 60.03 REPLICA 3 Ultra-Fine 0 8 312 105.53 0 2 48 80.89 Pyrethrum 04 110 105.2 0 0 0 58.96 Water 0 11 227 101.41 0 9 247 56.86 Formulation3 0 11 242 59.35 0 4 117 77.37 Ultra-Fine 0 0 12 18.92 0 1 0 23.48Pyrethrum 0 3 3 20.3 0 1 0 20.23 Water 0 1 19 26.25 0 6 76 32.28Formulation 4 0 2 38 16.83 0 2 16 15.03

TABLE 3 The Affect of Encapsulated Formulations on white fly Populationson Tomato Plants Treated Plants Non treated Plants Number of whitefliesNumber of whiteflies Formulation Leaf Top Leaf Bottom No. eggs Leaf TopLeaf Bottom No. eggs A 0 3 25 0 15 61 B 0 0 0 0 18 150 C 0 0 12 0 23 93D 0 5 0 0 18 35 E 0 2 10 0 15 64 F 0 10 44 0 11 21 G 0 12 20 0 10 39

For the next set of experiments, the following seven formulations wereprepared and used:

-   -   A. 95 ml cottonseed oil and 5 ml Tween    -   B. 24.4 ml cottonseed oil and 0.63 ml encapsulated ginger oil    -   C. 23.7 ml cottonseed oil and 1.2 ml encapsulated ginger oil    -   D. 22.5 ml cottonseed oil and 2.5 ml encapsulated ginger oil    -   E. 21.2 ml cottonseed oil and 3.75 ml encapsulated ginger oil    -   F. Ultra-Fine Oil    -   G. Water

The results of the experiments conducted respectful of repelling thewhitefly population from tomato plants are shown in Table 3. As may benoted, the formulations which were prepared in accordance with thepresent invention were much more effective in repelling whiteflies andin reducing the number of eggs laid.

What is claimed is:
 1. An essential oil formulation comprising: at leastone volatile essential oil, the at least one volatile essential oilbeing released from the essential oil formulation to provide itscharacteristic odor and a pest repelling, insecticidal, pesticidal,larvicidal and/or ovicidal effect; and a non-volatile vehicle in a solidor a liquid form, said non-volatile vehicle comprising a non-volatileoil, said at least one volatile essential oil being encapsulated andseparate from said non-volatile oil, wherein said non-volatile vehicleenhances the pest repelling, insecticidal, pesticidal and/or ovicidaleffect of the volatile essential oil, and wherein said non-volatile isselected from sesame oil, pyrethrum oil and combinations thereof.
 2. Theformulation of claim 1, wherein the essential oil is selected fromcinnamon, cedar, castor, clove, geranium, lemongrass, mint, thyme,turmeric, wintergreen, rosemary, anise, cardamom, chamomile, coriander,cumin, dill, mint, parsley, lavender, basil, camphor, citronella,eucalyptus, fennel, ginger, grapefruit, lemon, mandarin, orange, pineneedle, pepper, rose, sweet orange, tangerine, tea tree, tea seed,caraway, garlic, peppermint, onion, and spearmint.
 3. The formulation ofclaim 1, further comprising at least one additive selected from thegroup of adjuvants, adhesives, antioxidants, water-resistant agents,surfactants, steric barrier polymers and gel-breaking agents, as part ofthe vehicle or within the microcapsule.
 4. The formulation of claim 1,further comprising at least one agent selected from pesticides, insectgrowth regulators, herbicides, insecticides, acaracides, fungicides,nematicides, ectoparasiticides, and combinations thereto; wherein saidat least one agent is encapsulated with said at least one volatileessential oil.
 5. The formulation of claim 4, wherein said agent is apesticide selected from the group of carbamates, ureas, triazines,triazoles, uracils, organophosphates, morpholines, dinitroanilines,acylalanines, pyrethroids, organochlorines, carbofuran, azinphos-methyl,sulfentrazone, carfentrazone-ethyl, cypermethrin, cyromazine,beta-cyfluthrin, endosulfan, phosmet, chlorobromuron, chloroxuron,chlorotoluron, fluometuron, metobromuron, thiazafluron, teflubenzuron,hexaflumuron, diflubenzuron, flufenoxuron, lufenuron, chlorfluazuron,riovaluron, dimethachlor, metolachlor, pretilachlor,2-chloro-n-(l-methyl-2-methoxyethyl)-acet-2,6-xylidide, imidocloprid,alachlor, butachlor, propachlor, dimethenamid, bifenox,4-(4-pentyn-l-yloxy)diphenylether, acifluorfen, oxyfluorfen,fluoroglycofen-ethyl, fomesafen, cis,trans-(+)-2-ethyl-5-(4-phenoxyphenoxymethyl)-1,3-dioxolane,fluazifopbutyl, haloxyfop-methyl, haloxyfop-(2-ethoxyethyl), endosulfan,fluorotopic, fenoxapropethyl, quizalofop-ethyl, propaquizafop,diclofop-methyl, butralin, ethalfluralin, fluchloralin, isopropalin,pendimethalin, profluralin, trifluralin, aclalanines furalaxyl,metalaxyl, benzoylprop ethyl, flamprop methyl, difenoconazole,etaconazol, propiconazole,1,2-(2,4-dichlorophenyl)-pent-l-yl-1h-1,2,4-triazole, triadimefon,dioxacarb, furathiocarb, aldicarb, benomyl,2-sec-butylphenylmethylcarbamate, etiofencarb, fenoxycarb, isoprocarb,propoxur, carbetamid, butylate, di-allat, eptc, molinate, thiobencarb,tri-allate, vemolate, piperophos, anilofos, butamifos, azamethiphos,chlorfenvinphos, dichlorvos, diazinon, methidathion, azinphos ethyl,azinphos methyl, chlorpyrifos, chlorthiofos, crotoxyphos, cyanophos,demeton, dialifos, dimethoate, disulfoton, etrimfos, famphur,flusulfothion, fluthion, fonofos, formothion, heptenophos, isofen:phos,isoxathion, malathion, mephospholan, mevinphos, naled, oxydemetonmethyl, oxydeprofos, parathion, phoxim, pyrimiphos methyl, profenofos,propaphos, propetamphos, prothiophos, quinalphos, sulprofos, phemephos,terbufos, triazophos, trichloronate, fenamipos, isazophos, s-benzylo,o-diisopropylphosphorothioate, edinphos and pyrazophos.
 6. Theformulation of claim 1, wherein the formulation is in a preparation formselected from emulsifiable concentrate, wettable powder, granularwettable powder, flowable preparation, suspension, granule, dust,fumigant, solution, and aqueous solution.
 7. The formulation of claim 1,wherein the formulation is used to manage pest populations.
 8. Theformulation of claim 7, wherein the pest populations are selected fromwhiteflies, tomato pinworms, armyworms, stinkbugs pepper weevil pests orcombinations thereof.
 9. The formulation of claim 1, wherein theencapsulated volatile essential oils comprises a poly urea and/orpolyurethane film formed around said volatile essential oil.
 10. Theformulation of claim 1, wherein the non-volatile vehicle is notencapsulated together with said at least one volatile essential oil. 11.The formulation of claim 1, wherein the formulation is a two-componentformulation, wherein the at least one volatile essential oil is a firstcomponent and the non-volatile vehicle is a second component that isapplied separately from the first component.
 12. The formulation ofclaim 1, wherein said non-volatile oil is a mixture of sesame oil andpyrethrum oil.
 13. A method for managing a pest population, said methodcomprising applying to a target environment or to a pest population orto a loci thereof, a formulation according to claim
 1. 14. The methodaccording to claim 13, wherein said target environment is a primaryenvironment or a secondary environment.
 15. The method according toclaim 14, wherein said primary environment is selected from leaves,bark, fruits, flowers, seeds or roots of cereals, beans peas, fruittrees walnut, chestnut, almond, leafy vegetables, fruiting vegetables,root crops, processing crops, cucurbitaceous plants, pasture plants,lawn grasses, perfumery crops, ornamental plants, and timber woods. 16.A commercial package comprising the formulation according to claim 1.